LAUSR

Monochiral single‐walled carbon nanotubes (SWCNTs) are promising materials with potential applications in 3D integrated circuits and optoelectronic hybrid circuits. However, the purity and device performance of monochiral SWCNTs are still far lower than expected. Here, the authors demonstrate that specific monochiral SWCNTs can be wrapped by conjugated polymers containing pyridine units, and the supramolecular assemblies show surprising suspension stability even after high‐intensity ultracentrifugation. Additionally, two novel methods are developed, namely, enhanced ultracentrifugation (E‐UCG) and stepwise extraction processing (STEP), which successfully achieve isolation of (10,8) and (12,5) SWCNTs with respective diameters of 1.24 and 1.2 nm at high monochiral purity (92.3% and 95.6%). Their S11 absorption and fluorescence emission peaks are both at ≈1.5 µm (optical telecommunications C‐band). Both micro‐ and nanoscale field‐effect transistor (FET) devices can be fabricated from the as‐isolated (10,8) SWCNTs, and these FETs exhibit excellent electrical performance and a high semiconducting purity of up to 99.94%.